Unraveling the role of iron on Ni-Fe alloy nanoparticles during the electrocatalytic ethanol-to-acetate process  

作　　者：Junshan Li Luming Li Xinyu Ma Jun Wang Jun Zhao Yu Zhang Ren He Yaoyue Yang Andreu Cabot Yongfa Zhu 

机构地区：[1]Institute for Advanced Study,Chengdu University,610106 Chengdu,China [2]State Key Laboratory of Environmental-Friendly Energy Materials,Southwest University of Science and Technology,Mianyang 621010,China [3]College of Food and Biological Engineering,Chengdu University,Chengdu 610106,China [4]School of Chemistry and Environment,Southwest Minzu University,Chengdu 610041,China [5]Hebei Key Laboratory of Photoelectric Control on Surface and Interface,College of Science,Hebei University of Science and Technology,Shijiazhuang 050018,China [6]Catalonia Institute for Energy Research-IREC,Sant Adriàde Besòs,Barcelona 08930,Catalonia,Spain [7]ICREA,Pg.Lluís Companys 23,Barcelona 08010,Catalonia,Spain [8]Department of Chemistry,Tsinghua University,Beijing 100084,China

出　　处：《Nano Research》2024年第4期2328-2336,共9页纳米研究（英文版）

基　　金：supported by the Natural Science Foundation of Sichuan Province(No.2022NSFSC1229);the open project from Hebei Key Laboratory of Photoelectric Control on Surface and Interface(No.ZD2022003);J.S.L.thanks the project funded by China Postdoctoral Science Foundation(project No.2023MD734228);It was also supported by the European Regional Development Funds and by the Spanish Ministerio de Ciencia e Innovación through the project COMBENERGY(No.PID2019-105490RB-C32);Y.Y.Y.acknowledges funding from the National Natural Science Foundation of China(NSFC,No.22172121);the Fundamental Research Funds for the Central Universities,Southwest Minzu University(No.xiao2021102).

摘　　要：The anodic electrooxidation of ethanol to value-added acetate is an excellent example of replacing the oxygen evolution reaction to promote the cathodic hydrogen evolution reaction and save energy.Herein,we present a colloidal strategy to produce Ni-Fe bimetallic alloy nanoparticles(NPs)as efficient electrocatalysts for the electrooxidation of ethanol in alkaline media.Ni-Fe alloy NPs deliver a current density of 100 mA·cm^(-2) in a 1.0 M KOH solution containing 1.0 M ethanol merely at 1.5 V vs.reversible hydrogen electrode(RHE),well above the performance of other electrocatalysts in a similar system.Within continuous 10 h testing at this external potential,this electrode is able to produce an average of 0.49 mmol·cm^(-2)·h^(-1) of acetate with an ethanol-to-acetate Faradaic efficiency of 80%.A series of spectroscopy techniques are used to probe the electrocatalytic process and analyze the electrolyte.Additionally,density functional theory(DFT)calculations demonstrate that the iron in the alloy NPs significantly enhances the electroconductivity and electron transfer,shifts the rate-limiting step,and lowers the energy barrier during the ethanol-to-acetate reaction pathway.

关 键 词：ELECTROCATALYSIS ethanol oxidation reaction alloy nanoparticle ACETATE BIOREFINERY 

分 类 号：TG146[一般工业技术—材料科学与工程]